Engineering Ultrafine NiFe-LDH into Self-Supporting Nanosheets: Separation-and-Reunion Strategy to Expose Additional Edge Sites for Oxygen Evolution.

Here, a strategy is reported to prepare Ni-Fe layered double hydroxide (NiFe-LDH) with abundant exposed edge planes for enhanced oxygen evolution reaction (OER). The edge-to-edge assembly of ultrafine NiFe-LDH directed by graphite-like carbon is performed through a one-step hydrothermal process to form self-supporting nanosheet arrays (named NiFe-LDH/C), in which ascorbic acid is employed as the carbon precursor to control both the platelet size and the assembly mode of NiFe-LDH. Benefiting from the unique structural engineering, NiFe-LDH/C can not only achieve a fast surface reconstruction into the highly active γ-phase structure, but also exposes abundant active edge sites, thus leading to a superior OER performance with the overpotential as low as 234 mV at a current density of 50 mA cm . Furthermore, density functional theory (DFT) calculations reveal that the unsaturated Fe-sites and the bridge-sites connecting Ni and Fe atoms, which only exist on the edge planes of NiFe-LDH, are the main active centers responsible for promoting the intrinsic OER activity. This work provides a specific and valuable reference for the rational design of high-quality electrocatalysts through structural engineering for renewable energy applications.